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4/2003 Rev 2 I.4.9e – slide 1 of 100 Session I.4.9e Part I Review of Fundamentals Module 4Sources of Radiation Session 9eFuel Cycle - Enrichment IAEA Post Graduate Educational Course Radiation Protection and Safety of Radiation Sources
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4/2003 Rev 2 I.4.9e – slide 2 of 100 Enrichment
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4/2003 Rev 2 I.4.9e – slide 3 of 100 Why do Enrichment? Enriched uranium not necessary for nuclear reactors - can improve the moderation (carbon, D 2 O) which allows the use of natural uranium (e.g., CANDU, Magnox) Pure (enriched) isotopes offer enhanced properties and cleaner spectra for reactions
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4/2003 Rev 2 I.4.9e – slide 4 of 100 Possible Isotope Separation Methods “Physical” - Distillation- Thermal - Distillation- Thermal - Ion Exchange- Solvent Extraction - Ion Exchange- Solvent Extraction - Barrier Diffusion- Centrifugation - Barrier Diffusion- Centrifugation - Nozzle Flow- Helical Flow - Nozzle Flow- Helical Flow“Chemical” - Chemical Exchange - Chemical Exchange - Ionization - Ionization - Laser/Light - Laser/Light
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4/2003 Rev 2 I.4.9e – slide 5 of 100 Uranium Enrichment Methods Currently, two main methods implemented commercially Gaseous diffusion (GDP) Gas centrifuge (GC) Previous methods Thermal diffusion Electromagnetic ionization/Calutron Future Methods (?) - Both laser based AVLIS Silex In actual practice, theoretical enrichment values are rarely attained
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4/2003 Rev 2 I.4.9e – slide 6 of 100 Other Enrichment Definitions Enrichment Levels: LEU = Low Enriched Uranium: assay < 10% “IEU” = Intermediate Enriched Uranium (10% - 20%) HEU = High Enriched Uranium: assay > 20% (usually focus on assay > 90%) SWU = Separative Work Unit measure of physical effort in separation (cost) Enriched uranium is called Special Nuclear Material in the USA
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4/2003 Rev 2 I.4.9e – slide 7 of 100 Gaseous Diffusion Two enrichment processes: Gaseous Diffusion Gas Centrifuge
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4/2003 Rev 2 I.4.9e – slide 8 of 100 Basic Theory of Gaseous Diffusion Gaseous Diffusion uses molecular diffusion to separate the isotopes of uranium Three basic requirements are needed Combine Uranium with Fluorine to form Uranium hexafluoride (UF 6 ) Pass UF 6 through a porous membrane Utilize the different molecular velocities of the two isotopes to achieve separation
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4/2003 Rev 2 I.4.9e – slide 9 of 100 Enrichment of 235 U through one porous membrane (or barrier) is very minute Thousands of passes are required to increase the enrichment of natural uranium (0.711%) to a usable assay of 4 or 5% for use in reactors Basic Theory of Gaseous Diffusion
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4/2003 Rev 2 I.4.9e – slide 10 of 100 Eight-Step Program 1)UF 6 Feed Storage 2)Feed Supply Autoclave 3)Enrichment Cascade 4)Tails Condensation and Withdrawal 5)Tails Storage 6)Product Condensation and Withdrawal 7)Product Storage 8)Product Shipping
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4/2003 Rev 2 I.4.9e – slide 11 of 100 Step 1 - UF 6 Feed Storage Feed material typically arrives at a GDP via truck or rail Normal feed (i.e., natural uranium) can be received in 2.5, 10, and 14-ton cylinders UF 6 is in solid phase when being transported
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4/2003 Rev 2 I.4.9e – slide 12 of 100 Cylinder Filled with Solid UF 6
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4/2003 Rev 2 I.4.9e – slide 13 of 100 Step 2 - Feed Supply Autoclave Used to heat a cylinder to liquid phase Also acts as a containment Includes many safety systems Pressure Temperature Conductivity
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4/2003 Rev 2 I.4.9e – slide 14 of 100 Typical Autoclave UF 6 is liquefied and homogenized Sample drawn in order to check chemical purity and isotopic concentration
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4/2003 Rev 2 I.4.9e – slide 15 of 100 Phase Diagram of UF 6 Solid cylinder contents are heated to the liquid phase Fed into cascade as UF 6 gas Cylinder connected to cascade with a “pigtail”
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4/2003 Rev 2 I.4.9e – slide 16 of 100 Step 3 - Enrichment Cascade As mentioned earlier, the separation of 235 U from 238 U is accomplished by passing UF 6 through many hundreds of stages UF 6 flows into the stage, where it comes in contact with the porous surface of a barrier The barrier is what makes enrichment possible
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4/2003 Rev 2 I.4.9e – slide 17 of 100 Gaseous Diffusion Enrichment of 235 U through one porous membrane (or barrier) is very minute
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4/2003 Rev 2 I.4.9e – slide 18 of 100 Schematic of Diffusion Stage Some of the UF 6 (slightly more 235 U than 238 U) passes through to the low-pressure side of the converter High-pressure UF 6 gas stream passes through the barrier tubes
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4/2003 Rev 2 I.4.9e – slide 19 of 100 Product1.0 kg UF 6 at 3.0% 235 U Feed Depleted Uranium5.5 kgs UF 6 at 0.3% 235 U 6.5 kgs UF 6 at 0.711% 235 U Shape of a Cascade
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4/2003 Rev 2 I.4.9e – slide 20 of 100 SWU Cider Analogy Apples represent feed quantities Force represents Separative Work Unit or SWU (electricity/effort) Cider represents product (LEU) Peels/cores represent DU tails Relationship is non-linear but approximately linear in LEU range
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4/2003 Rev 2 I.4.9e – slide 21 of 100 SWU Cider Analogy Typical Feed (1 basket of apples) Waste (peels, cores, seeds, apples) Force(SWU) Less Feed More Force Feed (<1 basket) LessWaste MoreForce More Feed Less Force Feed (>1 basket) MoreWaste LessForce Product (1 liter cider) Same for all Three
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4/2003 Rev 2 I.4.9e – slide 22 of 100 Length of the Cascade Length is determined by the needed enrichment 5.0% enrichment requires many more stages than say 2.6% enrichment The number of stages required for a given enrichment can be calculated
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4/2003 Rev 2 I.4.9e – slide 23 of 100 Separation of 234 U Natural uranium also consists of a small quantity of 234 U Due to the process, 234 U gets enriched as well as 235 U Separation factor for 234 U = 1.006
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4/2003 Rev 2 I.4.9e – slide 24 of 100 Stages The entire cascade is composed of groups of stages
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4/2003 Rev 2 I.4.9e – slide 25 of 100 Step 4 – Tails Condensation and Withdrawal Tails are the depleted UF 6 stream UF 6 is compressed and condensed into a liquid Withdrawn into 10- or 14-ton cylinders Cooled at ambient conditions until UF 6 is solid, taking at least 5 days Typical assay of tails is between 0.2% and 0.4%
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4/2003 Rev 2 I.4.9e – slide 26 of 100 Step 5 – Tails Storage Stored on concrete storage yards Stacked two high Cylinder integrity is checked periodically Large equipment used to move cylinders is limited to only moving solid cylinders
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4/2003 Rev 2 I.4.9e – slide 27 of 100 Step 6 – Product Condensation and Withdrawal Enriched UF 6 is removed from the cascade through heated piping, where it is compressed and cooled to make it a liquid Put into 10-ton product cylinders Filled cylinders are moved to a cool down area for solidification Next, the gaseous contaminants are removed by “burping” them through chemical traps
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4/2003 Rev 2 I.4.9e – slide 28 of 100 Assay and Accumulation Assay in product cylinders can be determined by: Automatic sampler during filling In-line mass spectrometers UF 6 can be held-up in accumulators Allows uninterrupted filling of cylinders
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4/2003 Rev 2 I.4.9e – slide 29 of 100 Step 7 – Product Storage The 10-ton cylinders used for product withdrawal are not used for delivery Transferred to 2.5-ton cylinders Transferring allows the opportunity to confirm assay and purity of product
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4/2003 Rev 2 I.4.9e – slide 30 of 100 Step 8 – Product Shipping After a cylinder cools for 5 days, it can be shipped Loaded into overpacks Shipped via semi- truck
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4/2003 Rev 2 I.4.9e – slide 31 of 100 Potential Hazards Primary overall hazard is a major UF 6 release Liquid cylinder drop is most credible When UF 6 reacts with water, it forms hydrofluoric acid Both corrosive and toxic
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4/2003 Rev 2 I.4.9e – slide 32 of 100 UF 6 – Uranium Hexafluoride HF – Hydrogen Fluoride Cl 2 - Chlorine NH 3 - Ammonia ClF 3 – Chlorine Trifluoride Significant Hazards
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4/2003 Rev 2 I.4.9e – slide 33 of 100 Gas Centrifuge Two enrichment processes: Gaseous Diffusion Gas Centrifuge
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4/2003 Rev 2 I.4.9e – slide 34 of 100 Gas Centrifuges (GC) GC is a uranium enrichment process that uses a large number of rotating cylinders in series and parallel configurations to produce LEU suitable for commercial power reactor use The approach is a hundred years old Several large facilities overseas successfully and economically supply LEU using GC plants No operating GC plants currently exist in the U.S., but there have been “many discussions.”
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4/2003 Rev 2 I.4.9e – slide 35 of 100 Why Gas Centrifuge? Large enrichment effect per stage > 1.05 vs 1.004 for GDP More compact design Reduced uranium inventories in cascades Better energy efficiencies < 5% of GDP energy typically stated More rapidly achieves equilibrium/steady state about a day instead of “weeks” for GDP
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4/2003 Rev 2 I.4.9e – slide 36 of 100 Existing GC Plants and Capacities Urenco Plants: Capenhurst, UK: 2M SWU/yr, expanding to 2.5 Gronau, D: 1.3 M SWU/yr, expanding to ? Almelo, ND: 1.5 M SWU/yr, expanding to 2.5 Russia/FSU Several, 20 M SWU/yr Japan Several, circa 0.1 M SWU/yr, expanding to 1-1.5 M (Rokkasho-Mura, northern Honshu)
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4/2003 Rev 2 I.4.9e – slide 37 of 100 Gas Centrifuge Theory Slight density difference between 235 UF 6 and 238 UF 6 Separated by centrifugal forces created by rotation (20,000+ rpm) Enriched and depleted layers form Improve separation with countercurrent flow from baffles and thermal means (heat bottom, cool top) Improve separation and throughput with larger diameter and more height (DOE approach) Remove by scoops etc.
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4/2003 Rev 2 I.4.9e – slide 38 of 100 Gas Centrifuge
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4/2003 Rev 2 I.4.9e – slide 39 of 100 Unique Characteristics of GCs Rotors require high strength Super strong maraging steels Fiber (carbon) composites Supercritical operation rpm requires traversing natural harmonics, flexural nodes Bearings/drives must accommodate imperfections vibration during acceleration/deceleration drives must quickly traverse natural harmonics of the GC Many GCs required in plant (10,000s)
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4/2003 Rev 2 I.4.9e – slide 40 of 100 Gas Centrifuge (GC) Process Main operations and hazards similar to GDP UF 6 receive, store, desublime, “burp,” vaporize, product, tails, sample etc. Only the enrichment part changes GCs operate at lower pressure but higher separation Requires fewer stages in series (circa 50) Requires more stages in parallel to meet throughput Thus, organized in series and parallel cascades
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4/2003 Rev 2 I.4.9e – slide 41 of 100 Cascade Arrangement Note parallel and series arrangement
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4/2003 Rev 2 I.4.9e – slide 42 of 100 Gas Centrifuge Hazards Effect of high speed rotating equipment: 12” diameter rotor, at 350 m/sec edge speed Circumference is 0.94 m (i.e., per revolution) Result is 371 rev/sec = 22,300 rpm 82,000 g’s Increases in diameter, height, and rpm improve enrichment and production but also increase hazards and consequences of failures Compromises and trade-offs unavoidable and required
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4/2003 Rev 2 I.4.9e – slide 43 of 100 Safety Comparison: GC vs GDP Centrifuge Lower pressures, less inventory, more isolation Newer facility Liquid UF 6 areas comparable Conclude GC risk probably lower
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4/2003 Rev 2 I.4.9e – slide 44 of 100 Atomic Vapor Laser Isotope Separation (AVLIS)
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4/2003 Rev 2 I.4.9e – slide 45 of 100 AVLIS - Theory Focus on AVLIS process Uses uranium metal (actually U-Fe alloy - lower eutectic) Melt metal at circa 2,300 C in a vacuum chamber (separator or pod) – (for example Electron-beam) Forms U metal vapor “beam” between electrodes Visible, UV lasers form U-235+ ions, condense on cathode U-238 condenses on collector in back (and everywhere else!)
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4/2003 Rev 2 I.4.9e – slide 46 of 100 AVLIS - Theory Enriched product on collector
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4/2003 Rev 2 I.4.9e – slide 47 of 100 “The AVLIS Dilemmas” Batch processing Vacuum contradiction high vacuum to avoid collisions, improve selectivity low vacuum to improve throughput Collector design/fabrication ES&H Concerns temperature extremes (hot or cold) units/pods have to be opened more frequently than GDP internal coatings of U “stuff” - U metal/ Ux deposits intimate high energy equipment and lasers dense phases and criticality hot uranium is very corrosive and reactive
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4/2003 Rev 2 I.4.9e – slide 48 of 100 AVLIS - Potential Hazards Handling “molten” uranium Mixing of high energy components and water Unknown reliabilities - some analogues have high failure rates Fire hazards from dye lasers, reactions generating hydrogen Criticality due to dense phase - “nuggets” - and water Maintenance
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4/2003 Rev 2 I.4.9e – slide 49 of 100 SILEX Enrichment SILEX - Separation of Isotopes by Laser Excitation SILEX now known as GLE (Global Laser Enrichment) In mid-2009, GEH (GE – Hitachi) submitted the final part of its licence application to NRC If the licence application is successful and the decision to proceed is taken early in 2012, the GLE commercial production facility (at Wilmington, North Carolina) should be operational about 2014
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4/2003 Rev 2 I.4.9e – slide 50 of 100 What is Depleted Uranium? Definition: Depleted uranium (DU) is uranium that contains less than the natural assay of uranium-235 Natural assay = approximately 0.712% U-235 “Normal DU” is around 0.2-0.4% U-235 DU comes as a “byproduct” - some say “waste” - from enrichment
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4/2003 Rev 2 I.4.9e – slide 51 of 100 DU Background Generated by every enrichment process DU generation cannot be avoided minimum of about 5:1 ratio to LEU product ratio of 8-10:1 due to higher assays, more U feed Perceived hazards old and rusting containers chemical - UF 6, F 2 liability for cleanup, accidents
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4/2003 Rev 2 I.4.9e – slide 52 of 100 What are the potential hazards with DUF 6 ? DU’s chemical toxicity greater than its radiotoxicity heavy metal ingestion equivalent to about 10 mSv dose can be fatal DUF 6 readily reacts with atmospheric water vapor to form UO 2 F 2 and HF (both “bad”) DUF 6 corrosive (+ HF effect) DUF 6 reacts violently with most organic materials For any DU disposition/plant alternative: large quantities, liquid UF 6, high temps, airborne concern, fluorine/HF disposition
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4/2003 Rev 2 I.4.9e – slide 53 of 100 DU Current Approach and Programs Store as UF 6 solid in 48” cylinders (48G) outside U.S./DOE: Inspect/Maintain/Paint cylinders about 6 small leaks/leakers in 50,000 cylinders, over 40 years DOE has title to most U.S. DUF 6 USEC payment for DOE to accept DUF 6 Overseas Most countries store DU as DUF 6 Only France converts DUF 6 to DU 3 O 8 powder
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